Review: using rolled-up tubes for strain-tuning the optical properties of quantum emitters.

Rolled-up tubes based on released III-V heterostructures have been extensively studied and established as optical resonators in the last two decades. In this review, we discuss how light emitters (quantum wells and quantum dots) are influenced by the inherently asymmetric strain state of these tubes. Therefore, we briefly review whispering gallery mode resonators built from rolled-up III-V heterostructures. The curvature and its influence over the diameter of the rolled-up micro- and nanotubes are discussed, with emphasis on the different possible strain states that can be produced. Experimental techniques that access structural parameters are essential to obtain a complete and correct image of the strain state for the emitters inside the tube wall. In order to unambiguously extract such strain state, we discuss x-ray diffraction results in these systems, providing a much clearer scenario compared to a sole tube diameter analysis, which provides only a first indication of the lattice relaxation in a given tube. Further, the influence of the overall strain lattice state on the band structure is examined via numerical calculations. Finally, experimental results for the wavelength shift of emissions due to the tube strain state are presented and compared with theoretical calculations available in literature, showing that the possibility to use rolled-up tubes to permanently strain engineer the optical properties of build-in emitters is a consistent method to induce the appearance of electronic states unachievable by direct growth methods.

Acoustically Driven Stark Effect in Transition Metal Dichalcogenide Monolayers.

The Stark effect is one of the most efficient mechanisms to manipulate many-body states in nanostructured systems. In mono- and few-layer transition metal dichalcogenides, it has been successfully induced by optical and electric field means. Here, we tune the optical emission energies and dissociate excitonic states in MoSe2 monolayers employing the 220 MHz in-plane piezoelectric field carried by surface acoustic waves. We transfer the monolayers to high dielectric constant piezoelectric substrates, where the neutral exciton binding energy is reduced, allowing us to efficiently quench (above 90%) and red-shift the excitonic optical emissions. A model for the acoustically induced Stark effect yields neutral exciton and trion in-plane polarizabilities of 530 and 630 × 10-5 meV/(kV/cm)2, respectively, which are considerably larger than those reported for monolayers encapsulated in hexagonal boron nitride. Large in-plane polarizabilities are an attractive ingredient to manipulate and modulate multiexciton interactions in two-dimensional semiconductor nanostructures for optoelectronic applications.

Author Correction: Optical Absorption Exhibits Pseudo-Direct Band Gap of Wurtzite Gallium Phosphide.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Optical Absorption Exhibits Pseudo-Direct Band Gap of Wurtzite Gallium Phosphide.

Definitive evidence for the direct band gap predicted for Wurtzite Gallium Phosphide (WZ GaP) nanowires has remained elusive due to the lack of strong band-to-band luminescence in these materials. In order to circumvent this problem, we successfully obtained large volume WZ GaP structures grown by nanoparticle-crawling assisted Vapor-Liquid-Solid method. With these structures, we were able to observe bound exciton recombination at 2.14 eV with FHWM of approximately 1 meV. In addition, we have measured the optical absorption edges using photoluminescence excitation spectroscopy. Our results show a 10 K band gap at 2.19 eV and indicate a weak oscillator strength for the lowest energy band-to-band absorption edge, which is a characteristic feature of a pseudo-direct band gap semiconductor. Furthermore, the valence band splitting energies are estimated as 110 meV and 30 meV for the three highest bands. Electronic band structure calculations using the HSE06 hybrid density functional agree qualitatively with the valence band splitting energies.

Band structure engineering in strain-free GaAs mesoscopic systems.

We investigate the optical properties of strain-free mesoscopic GaAs/Al x Ga1 - x As structures (MGS) coupled to thin GaAs/Al x Ga1 - x As quantum wells (QWs) with varying Al content (x). We demonstrate that quenching the QW emission by controlling the band crossover between AlGaAs (X-point) and GaAs (Γ-point) gives rise to long carrier lifetimes and enhanced optical emission from the MGS. For x = 0.33, QW and MGS show typical type-I band alignment with strong QW photoluminescence emission and much weaker sharp recombination lines from the MGS localized exciton states. For x ≥ 0.50, the QW emission is considerably quenched due to the change from type-I to type-II structure while the MGS emission is enhanced due to carrier injection from the QW. For x ≥ 0.70, we observe PL quenching from the MGS higher energy states also due to the crossover of X and Γ bands, demonstrating spectral filtering of the MGS emission. Time-resolved measurements reveal two recombination processes in the MGS emission dynamics. The fast component depends mainly on the X - Γ mixing of the MGS states and can be increased from 0.3 to 2.5 ns by changing the Al content. The slower component, however, depends on the X - Γ mixing of the QW states and is associated to the carrier injection rate from the QW reservoir into the MGS structure. In this way, the independent tuning of X - Γ mixing in QW and MGS states allows us to manipulate recombination rates in the MGS as well as to make carrier injection and light extraction more efficient.

A Luminescent Thermometer Exhibiting Slow Relaxation of the Magnetization: Toward Self-Monitored Building Blocks for Next-Generation Optomagnetic Devices.

The development and integration of Single-Molecule Magnets (SMMs) into molecular electronic devices continue to be an exciting challenge. In such potential devices, heat generation due to the electric current is a critical issue that has to be considered upon device fabrication. To read out accurately the temperature at the submicrometer spatial range, new multifunctional SMMs need to be developed. Herein, we present the first self-calibrated molecular thermometer with SMM properties, which provides an elegant avenue to address these issues. The employment of 2,2'-bipyrimidine and 1,1,1-trifluoroacetylacetonate ligands results in a dinuclear compound, [Dy2(bpm)(tfaa)6], which exhibits slow relaxation of the magnetization along with remarkable photoluminescent properties. This combination allows the gaining of fundamental insight in the electronic properties of the compound and investigation of optomagnetic cross-effects (Zeeman effect). Importantly, spectral variations stemming from two distinct thermal-dependent mechanisms taking place at the molecular level are used to perform luminescence thermometry over the 5-398 K temperature range. Overall, these properties make the proposed system a unique molecular luminescent thermometer bearing SMM properties, which preserves its temperature self-monitoring capability even under applied magnetic fields.

Exploring Au Droplet Motion in Nanowire Growth: A Simple Route toward Asymmetric GaP Morphologies.

Here we show a new nanowire growth procedure, exploring the thermally activated motion of Au droplets on III-V surfaces. We show that by setting a single growth parameter we can activate the crawling motion of Au droplets in vacuum and locally modify surface composition in order to enhance vapor-solid (VS) growth along oxide-free areas on the trail of the metal particle. Asymmetric VS growth rates are comparable in magnitude to the vapor-liquid-solid growth, producing unconventional wurtzite GaP morphologies, which shows negligible defect density as well as optical signal in the green spectral region. Finally, we demonstrate that this effect can also be explored in different substrate compositions and orientations with the final shape finely tuned by group III flow and nanoparticle size. This distinct morphology for wurtzite GaP nanomaterials can be interesting for the design of nanophotonics devices.

Fabrication and Optical Properties of Strain-free Self-assembled Mesoscopic GaAs Structures.

We use a combined process of Ga-assisted deoxidation and local droplet etching to fabricate unstrained mesoscopic GaAs/AlGaAs structures exhibiting a high shape anisotropy with a length up to 1.2 µm and a width of 150 nm. We demonstrate good controllability over size and morphology of the mesoscopic structures by tuning the growth parameters. Our growth method yields structures, which are coupled to a surrounding quantum well and present unique optical emission features. Microscopic and optical analysis of single structures allows us to demonstrate that single structure emission originates from two different confinement regions, which are spectrally separated and show sharp excitonic lines. Photoluminescence is detected up to room temperature making the structures the ideal candidates for strain-free light emitting/detecting devices.